In femtosecond magnetism, a femtosecond laser pulse affects the spin moment only indirectly through the orbital angular momentum and the spin–orbit coupling. A long-standing puzzle is what happens if the orbital angular momentum itself is quenched. Here, we employ a four-level system to resolve this puzzle. The results show that the quenching of the orbital angular moment in the ground state has no direct relation to the spin moment change. By contrast, the orbital moment can be restored partially after the pulsed optical excitation and can affect the demagnetization. Importantly, this study confirms that the orbital moment indeed responds to the laser field faster than spin if the pulse duration is short, consistent with the recent time-resolved X-ray magnetic circular dichroism experiment. Therefore, our finding shines new light on femtosecond magnetism.
Switchable X-Ray Orbital Angular Momentum from an Artificial Spin Ice